CN103199277B - Sulfate treatment system with in-situ utilization of electricity of microbial fuel cell and application method of sulfate treatment system - Google Patents
Sulfate treatment system with in-situ utilization of electricity of microbial fuel cell and application method of sulfate treatment system Download PDFInfo
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- 230000000813 microbial effect Effects 0.000 title claims abstract description 72
- 238000000034 method Methods 0.000 title claims abstract description 26
- 238000011065 in-situ storage Methods 0.000 title abstract description 17
- 230000005611 electricity Effects 0.000 title description 5
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims abstract description 122
- 229910052717 sulfur Inorganic materials 0.000 claims abstract description 78
- 239000011593 sulfur Substances 0.000 claims abstract description 78
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- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 20
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- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 14
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- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
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- -1 SO 4 2- Chemical class 0.000 description 1
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
一种微生物燃料电池电能原位利用的硫酸盐处理系统及其使用方法，它涉及一种微生物燃料电池处理系统。本发明要解决现有的含硫废水微生物燃料电池系统中生成的单质硫附着在微生物燃料电池阳极极板上，影响阳极的生物电化学性能、且单质硫难于回收的问题。本发明系统由硫酸盐还原微生物燃料电池系统、电池升压模块系统和电化学硫氧化系统构成，通过微生物燃料电池系统产生电能，输送至电池升压模块系统进行贮存和转化，利用来自升压模块储存的电能驱动电化学硫氧化系统，将S2-转化为单质硫。本发明具有运行成本低、操作条件方便等优势，并可有效的回收单质硫资源，是集污水处理、能量、资源回收利用于一体的处理工艺，具有广阔的应用前景。
The invention relates to a sulfate treatment system for in-situ utilization of microbial fuel cell electric energy and a method for using the same, which relates to a microbial fuel cell treatment system. The invention aims to solve the problems that the elemental sulfur generated in the existing sulfur-containing wastewater microbial fuel cell system adheres to the anode plate of the microbial fuel cell, affects the bioelectrochemical performance of the anode, and is difficult to recycle the elemental sulfur. The system of the present invention is composed of a sulfate reducing microbial fuel cell system, a battery boost module system and an electrochemical sulfur oxidation system. Electric energy is generated by the microbial fuel cell system and delivered to the battery boost module system for storage and conversion. The stored electrical energy drives an electrochemical sulfur oxidation system to convert S2- into elemental sulfur. The invention has the advantages of low operating cost and convenient operating conditions, and can effectively recover elemental sulfur resources. It is a treatment process integrating sewage treatment, energy, and resource recovery and utilization, and has broad application prospects.
Description
技术领域technical field
本发明涉及一种微生物燃料电池系统及其使用方法。The invention relates to a microbial fuel cell system and its application method.
背景技术Background technique
随着我国工业的迅猛发展，特别是一些重污染行业，在生产过程中，会产生大量的含硫废水。据统计数据显示，我国涉及含硫的制药、化工等各类工业企业已超过了5万户，排放的含硫有机污水废水量超过60亿吨，同时，这类含硫废水中硫污染物浓度高、毒性大、易腐蚀废水构筑物、且处理往往无法达标，因此，含硫废水亟待处理。With the rapid development of my country's industry, especially in some heavily polluting industries, a large amount of sulfur-containing wastewater will be produced in the production process. According to statistical data, there are more than 50,000 industrial enterprises involved in sulfur-containing pharmaceuticals and chemicals in my country, and the amount of sulfur-containing organic wastewater discharged exceeds 6 billion tons. At the same time, the concentration of sulfur pollutants in such sulfur-containing wastewater High, high toxicity, easy to corrode wastewater structures, and the treatment is often not up to standard, therefore, sulfur-containing wastewater needs to be treated urgently.
含硫废水中往往含有多种硫化合物，其中包括：SO4 2-、HS-、S2-等多种形态，不同的硫化物进入到环境水体中后，会导致环境水体水质严重恶化。当含硫化合物在厌氧条件下会被微生物还原，产生有毒气体硫化氢，会引起生物腐蚀，且气味恶臭，对人体健康及大气环境污染严重；未处理完全的硫酸盐废水排入水体环境后，会造成水体pH值降低、土壤酸化、对水体及水生生物产生严重污染，影响受纳水体的生态环境安全。同时，如果未经处理的含硫废水进入到传统的废水处理系统后，会对废水构筑物的正常运转产生很大影响，因此，急需对含硫废水进行有效的去除，从而从根本上解决含硫废水带来的严重环境污染问题。Sulfur-containing wastewater often contains a variety of sulfur compounds, including: SO 4 2- , HS - , S 2- and other forms. When different sulfides enter the environmental water body, the water quality of the environmental water body will be seriously deteriorated. When sulfur-containing compounds are reduced by microorganisms under anaerobic conditions, toxic gas hydrogen sulfide will be produced, which will cause biological corrosion, and the smell is foul, which will seriously pollute human health and the atmospheric environment; after the untreated sulfate wastewater is discharged into the water environment , will cause the pH value of the water body to decrease, soil acidification, serious pollution to the water body and aquatic organisms, and affect the ecological environment safety of the receiving water body. At the same time, if untreated sulfur-containing wastewater enters the traditional wastewater treatment system, it will have a great impact on the normal operation of wastewater structures. Therefore, it is urgent to effectively remove sulfur-containing wastewater to fundamentally solve the problem of sulfur-containing wastewater. Serious environmental pollution caused by waste water.
传统的含硫废水处理方法通常采用物化方法和生化方法等2类处理方法进行，物化方法由于在处理过程中会增加额外的能耗并引入其他的化学试剂，因此，还需要进行后续的二次处理，而生化方法由于具有反应条件温和，操作条件简便、无需二次处理，因而被广泛的使用。在生化处理方法中，由于处理后产生的单质硫往往和污泥结合，收集具有较大的困难，从而使得系统中的单质硫回收率低，因此，如何在降低系统的运行成本的同时将产生的单质硫有效地回收是含硫废水生化处理过程的一个关键问题。Traditional sulfur-containing wastewater treatment methods usually use two types of treatment methods, such as physical and chemical methods and biochemical methods. Physical and chemical methods will increase additional energy consumption and introduce other chemical reagents during the treatment process. Therefore, subsequent secondary treatment is required. Biochemical methods are widely used because of their mild reaction conditions, simple operating conditions, and no need for secondary treatment. In the biochemical treatment method, since the elemental sulfur produced after treatment is often combined with sludge, it is difficult to collect, which makes the recovery rate of elemental sulfur in the system low. Therefore, how to reduce the operating cost of the system and at the same time generate The efficient recovery of elemental sulfur is a key issue in the biochemical treatment of sulfur-containing wastewater.
微生物燃料电池技术是环境工程领域近年来新兴的废水处理手段。微生物燃料电池技术是通过微生物作为催化剂，将废水中的有机底物进行分解代谢，同时将底物中的化学能转化为电子、质子，电子通过外电路传递到微生物燃料电池系统的阴极，质子通过内电路到达阴极，电子、质子和阴极的最终电子受体进行结合，完成最终的反应过程。通过微生物燃料电池系统，可以从有机废水中提取清洁能源电能，因此，微生物燃料电池技术是可以实现废水能源化的有效手段。微生物燃料电池系统作为一个生物处理过程，同样可以处理含硫废水，但是微生物燃料电池系统同样存在着单质硫难于回收的难题，为有效的解决单质硫的回收问题，急需对现有的微生物燃料电池系统进行改造。Microbial fuel cell technology is an emerging wastewater treatment method in the field of environmental engineering in recent years. Microbial fuel cell technology uses microorganisms as catalysts to decompose and metabolize the organic substrates in wastewater, and at the same time convert the chemical energy in the substrates into electrons and protons. The electrons are transferred to the cathode of the microbial fuel cell system through an external circuit, and the protons pass through The inner circuit reaches the cathode, and electrons, protons and the final electron acceptor of the cathode are combined to complete the final reaction process. Through the microbial fuel cell system, clean energy and electric energy can be extracted from organic wastewater. Therefore, microbial fuel cell technology is an effective means to realize the energy conversion of wastewater. As a biological treatment process, the microbial fuel cell system can also treat sulfur-containing wastewater, but the microbial fuel cell system also has the difficulty of recovering elemental sulfur. In order to effectively solve the problem of elemental sulfur recovery, there is an urgent need for existing microbial fuel cell The system is modified.
发明内容Contents of the invention
本发明的目的是为了解决现有含硫有机废水处理中存在的能源消耗、运行成本高及单质硫回收率低的问题，而提供了一种微生物燃料电池电能原位利用的硫酸盐处理系统及其使用方法。The object of the present invention is to provide a sulfate treatment system and How to use it.
本发明的一种微生物燃料电池电能原位利用的硫酸盐处理系统，由硫酸盐还原微生物燃料电池系统、电池升压模块系统和电化学硫氧化系统构成，硫酸盐还原微生物燃料电池系统与电化学硫氧化系统分别通过外部导线与电池升压模块系统连接；A sulfate treatment system for in-situ utilization of microbial fuel cell electric energy of the present invention is composed of a sulfate reducing microbial fuel cell system, a battery boost module system and an electrochemical sulfur oxidation system. The sulfate reducing microbial fuel cell system and electrochemical The sulfur oxidation system is respectively connected to the battery booster module system through external wires;
所述的硫酸盐还原微生物燃料电池系统由阳极盖板、阳极电极、阴极电极、阴极盖板、进水口和出水口构成；其中，硫酸盐还原微生物燃料电池系统底端和上端密封，硫酸盐还原微生物燃料电池系统上端设置有进水口和出水口；阳极盖板与阳极电极通过硅胶垫片进行密封连接，阴极盖板与阴极电极通过硅胶垫片进行密封连接，阳极电极、阴极电极分别与钛丝相连，并通过硅胶垫片进行密封连接，钛丝通过外部导线与电池升压模块系统连接；The sulfate-reducing microbial fuel cell system is composed of an anode cover plate, an anode electrode, a cathode electrode, a cathode cover plate, a water inlet and a water outlet; wherein, the bottom and upper ends of the sulfate-reducing microbial fuel cell system are sealed, and the sulfate reduction The upper end of the microbial fuel cell system is provided with a water inlet and a water outlet; the anode cover plate and the anode electrode are sealed and connected through a silica gel gasket, the cathode cover plate and the cathode electrode are sealed and connected through a silica gel gasket, and the anode electrode and the cathode electrode are respectively connected to the titanium wire. Connected and sealed through a silicone gasket, the titanium wire is connected to the battery booster module system through an external wire;
所述的电化学硫氧化系统由阳极盖板、阳极电极、阴极电极、阴极盖板、进水口和出水口构成，其中，电化学硫氧化系统底端和上端密封，电化学硫氧化系统上端设置有进水口和出水口；阳极盖板与阳极电极通过硅胶垫片进行密封连接，阴极盖板与阴极电极通过硅胶垫片进行密封连接，阳极电极与阴极电极分别与钛丝相连，并通过硅胶垫片进行密封连接，钛丝通过外部导线与电池升压模块系统连接。The electrochemical sulfur oxidation system is composed of an anode cover plate, an anode electrode, a cathode electrode, a cathode cover plate, a water inlet and a water outlet, wherein the bottom and upper ends of the electrochemical sulfur oxidation system are sealed, and the upper end of the electrochemical sulfur oxidation system is set There are water inlet and water outlet; the anode cover plate and the anode electrode are sealed and connected through the silicone gasket, the cathode cover plate and the cathode electrode are sealed and connected through the silicone gasket, the anode electrode and the cathode electrode are respectively connected to the titanium wire, and are connected through the silicone gasket The sheets are sealed and connected, and the titanium wire is connected to the battery booster module system through external wires.
本发明的一种微生物燃料电池电能原位利用的硫酸盐处理系统的操作方法如下：将含硫废水通过进水口注入到硫酸盐还原微生物燃料电池系统中，在设定的固定外阻下，启动硫酸盐还原微生物燃料电池，利用该系统中的硫酸盐还原菌代谢硫酸盐，将硫酸盐转化成硫化物，产生的电能通过电池升压模块系统进行能量的收集和捕获，存储和利用，将硫酸盐还原微生物燃料电池系统中处理的出水通过出水口注入到电化学硫氧化系统中，利用来自升压模块系统储存的电能，驱动电化学硫氧化系统，实现能量的自供给和利用，从而实现硫化物向单质硫的转化。The operation method of the sulfate treatment system for the in-situ utilization of microbial fuel cell electric energy of the present invention is as follows: inject sulfur-containing wastewater into the sulfate reducing microbial fuel cell system through the water inlet, and start the system under a set fixed external resistance Sulfate-reducing microbial fuel cells use the sulfate-reducing bacteria in the system to metabolize sulfate, convert sulfate into sulfide, and generate electricity through the battery booster module system for energy collection and capture, storage and utilization, and sulfuric acid The effluent treated in the salt-reducing microbial fuel cell system is injected into the electrochemical sulfur oxidation system through the water outlet, and the electric energy stored in the booster module system is used to drive the electrochemical sulfur oxidation system to realize self-supply and utilization of energy, thereby realizing vulcanization conversion to elemental sulfur.
本发明包含以下有益效果：The present invention comprises following beneficial effect:
本发明为克服含硫有机废水处理中存在的能源消耗、运行成本高及单质硫回收率低的技术难点，以降低系统的能源消耗、运行成本、提高单质硫的回收率为目的，构建了微生物燃料电池电能原位利用的含硫废水处理系统。该系统可以在室温下运行，硫酸盐去除率可达89%，单质硫回收率可达46%。通过该系统中的升压模块系统，可以在无外加能量输入的情况下，驱动电化学硫氧化系统实现硫化物向单质硫的转化，从而实现了电能的原位利用。该系统解决了含硫废水处理过程中的高能耗、低单质硫回收率问题，实现了含硫废水的资源化及能源化利用。本发明可利用系统中自身产生的能量来驱动电化学系统，因此，本系统是一个能量零消耗的处理系统，可适用于实际含硫废水的处理。In order to overcome the technical difficulties of energy consumption, high operating cost and low recovery rate of elemental sulfur in the treatment of sulfur-containing organic wastewater, the present invention constructs a microbial A sulfur-containing wastewater treatment system utilizing fuel cell electricity in situ. The system can operate at room temperature, the sulfate removal rate can reach 89%, and the elemental sulfur recovery rate can reach 46%. Through the step-up module system in the system, the electrochemical sulfur oxidation system can be driven to realize the conversion of sulfide to elemental sulfur without external energy input, thereby realizing the in-situ utilization of electric energy. The system solves the problems of high energy consumption and low recovery rate of elemental sulfur in the treatment process of sulfur-containing wastewater, and realizes the resource utilization and energy utilization of sulfur-containing wastewater. The present invention can use the energy generated by the system itself to drive the electrochemical system. Therefore, the system is a treatment system with zero energy consumption and is applicable to the treatment of actual sulfur-containing wastewater.
本发明的微生物燃料电池电能原位利用的含硫废水处理系统的运行方式如下：该系统由3部分组成，其3组分的运行模式分别为：The operating mode of the sulfur-containing wastewater treatment system utilizing microbial fuel cell electric energy in situ of the present invention is as follows: the system is composed of 3 parts, and the operating modes of the 3 components are respectively:
硫酸盐还原系统：以稳定运行的微生物燃料电池反应器的出水作为菌源，启动硫酸盐还原微生物燃料电池，阴阳极间以设定的外电阻启动（100-1000Ω），监测系统的电压输出情况，当输出电压稳定运行后（输出电压的在2-3个周期内达到稳定），向系统中添加市售的硫酸盐还原细菌作为硫酸盐还原系统的菌源，利用市售的硫酸盐还原细菌还原系统中的硫酸盐，利用产电细菌，在微生物燃料电池系统中获得电能。产生的电能输入到电池升压模块系统中进行贮存和累积。Sulfate reduction system: use the effluent of the microbial fuel cell reactor in stable operation as the bacterial source, start the sulfate reduction microbial fuel cell, start with the set external resistance (100-1000Ω) between the cathode and anode, and monitor the voltage output of the system , when the output voltage runs stably (the output voltage reaches stability within 2-3 cycles), add commercially available sulfate-reducing bacteria to the system as the bacterial source of the sulfate-reducing system, and use commercially available sulfate-reducing bacteria Reduction of sulfate in the system and use of electrogenic bacteria to obtain electrical energy in microbial fuel cell systems. The generated electrical energy is input into the battery booster module system for storage and accumulation.
电池升压模块系统：由计时继电器、电容等组成。通过计时继电器来控制电容器的充、放电的时间。利用不同容量的电容器以及不同数量的电容器，对硫酸盐还原微生物燃料电池系统产生的能量进行累加，以达到电化学硫氧化系统所需要的能量需求。Battery boost module system: composed of timing relays, capacitors, etc. The charging and discharging time of the capacitor is controlled by a timing relay. Capacitors with different capacities and different numbers of capacitors are used to accumulate the energy generated by the sulfate reduction microbial fuel cell system to meet the energy demand required by the electrochemical sulfur oxidation system.
电化学硫氧化系统：该系统为电化学反应系统，该系统由阳极、阴极和电解液组成。电解液为硫酸盐还原系统的出水。通过电池升压模块系统对硫酸盐还原系统收集的电能进行贮存和转化后，将升压模块系统作为外部电源供给到电化学硫氧化系统中，利用阳极发生的反应将电化学硫氧化系统中的S2-转化为单质硫。单质硫富集在阳极极板上，以便于快速收集产生的单质硫。Electrochemical sulfur oxidation system: This system is an electrochemical reaction system, which is composed of anode, cathode and electrolyte. The electrolyte is the effluent of the sulfate reduction system. After storing and converting the electric energy collected by the sulfate reduction system through the battery booster module system, the booster module system is used as an external power supply to the electrochemical sulfur oxidation system, and the reaction in the anode is used to convert the electric energy in the electrochemical sulfur oxidation system S 2- is converted to elemental sulfur. Elemental sulfur is enriched on the anode plate, so that the generated elemental sulfur can be collected quickly.
附图说明Description of drawings
图1为微生物燃料电池电能原位利用的含硫废水处理系统示意图；Figure 1 is a schematic diagram of a sulfur-containing wastewater treatment system utilizing microbial fuel cell electric energy in situ;
图2为实施例1中不同批次的COD降解率柱状图，其中，为A1批次的COD降解率柱状图，为A2批次的COD降解率柱状图，为A3批次的COD降解率柱状图；Fig. 2 is the COD degradation rate histogram of different batches in embodiment 1, wherein, is the histogram of the COD degradation rate of the A1 batch, It is the histogram of the COD degradation rate of the A2 batch, It is the histogram of the COD degradation rate of the A3 batch;
图3为实施例2中不同批次的硫酸盐去除率柱状图，其中，为A1批次的硫酸盐去除率柱状图，为A2批次的硫酸盐去除率柱状图，为A3批次的硫酸盐去除率柱状图；Fig. 3 is the bar chart of the sulfate removal rate of different batches in embodiment 2, wherein, is the sulfate removal rate histogram of the A1 batch, is the sulfate removal rate histogram of the A2 batch, It is the histogram of the sulfate removal rate of the A3 batch;
图4为实施例3中不同的升压模块获得的放电曲线图，其中，为YM-1升压模块获得的放电曲线图，为YM-2升压模块获得的放电曲线图，为YM-3升压模块获得的放电曲线图，为YM-4升压模块获得的放电曲线图；Fig. 4 is a discharge curve obtained by different boost modules in embodiment 3, wherein, The discharge curve graph obtained for the YM-1 boost module, The discharge curve graph obtained for the YM-2 boost module, The discharge curve graph obtained for the YM-3 boost module, The discharge curve graph obtained for the YM-4 boost module;
图5为实施例4中不同批次的单质硫回收率柱状图，其中，为A1批次的单质硫回收率柱状图，为A2批次的单质硫回收率柱状图，为A3批次的单质硫回收率柱状图。Fig. 5 is the bar chart of elemental sulfur recovery rate of different batches in embodiment 4, wherein, is the histogram of the elemental sulfur recovery rate of the A1 batch, is the histogram of the elemental sulfur recovery rate of the A2 batch, It is the histogram of elemental sulfur recovery rate of batch A3.
具体实施方式Detailed ways
具体实施方式一：本实施方式的一种微生物燃料电池电能原位利用的硫酸盐处理系统，由硫酸盐还原微生物燃料电池系统1、电池升压模块系统2和电化学硫氧化系统3构成，硫酸盐还原微生物燃料电池系统1与电化学硫氧化系统3分别通过外部导线18与电池升压模块系统2连接；Embodiment 1: A sulfate treatment system for in-situ utilization of microbial fuel cell electric energy in this embodiment is composed of a sulfate reducing microbial fuel cell system 1, a battery boost module system 2 and an electrochemical sulfur oxidation system 3. Sulfuric acid The salt-reducing microbial fuel cell system 1 and the electrochemical sulfur oxidation system 3 are respectively connected to the battery booster module system 2 through external wires 18;
所述的硫酸盐还原微生物燃料电池系统1由阳极盖板4、阳极电极5、阴极电极6、阴极盖板7、进水口8和出水口9构成；其中，硫酸盐还原微生物燃料电池系统1底端和上端密封，硫酸盐还原微生物燃料电池系统1上端设置有进水口8和出水口9；阳极盖板4与阳极电极5通过硅胶垫片进行密封连接，阴极盖板7与阴极电极6通过硅胶垫片进行密封连接，阳极电极5、阴极电极6分别与钛丝19，20相连，并通过硅胶垫片进行密封连接，钛丝19，20通过外部导线18与电池升压模块系统2连接；The sulfate reducing microbial fuel cell system 1 is composed of an anode cover plate 4, an anode electrode 5, a cathode electrode 6, a cathode cover plate 7, a water inlet 8 and a water outlet 9; wherein, the sulfate reducing microbial fuel cell system 1 bottom The end and the upper end are sealed, and the upper end of the sulfate reducing microbial fuel cell system 1 is provided with a water inlet 8 and a water outlet 9; the anode cover plate 4 and the anode electrode 5 are sealed and connected through a silica gel gasket, and the cathode cover plate 7 and the cathode electrode 6 are connected through a silica gel gasket. Gaskets are sealed and connected, the anode electrode 5 and the cathode electrode 6 are connected to titanium wires 19 and 20 respectively, and are sealed and connected through silica gel gaskets, and the titanium wires 19 and 20 are connected to the battery booster module system 2 through external wires 18;
所述的电化学硫氧化系统3由阳极盖板10、阳极电极11、阴极电极12、阴极盖板13、进水口14和出水口15构成，其中，电化学硫氧化系统3底端和上端密封，电化学硫氧化系统3上端设置有进水口14和出水口15；阳极盖板10与阳极电极11通过硅胶垫片进行密封连接，阴极盖板13与阴极电极12通过硅胶垫片进行密封连接，阳极电极11与阴极电极12分别与钛丝21，22相连，并通过硅胶垫片进行密封连接，钛丝21，22通过外部导线18与电池升压模块系统2连接。The electrochemical sulfur oxidation system 3 is composed of an anode cover plate 10, an anode electrode 11, a cathode electrode 12, a cathode cover plate 13, a water inlet 14 and a water outlet 15, wherein the bottom end and the upper end of the electrochemical sulfur oxidation system 3 are sealed The upper end of the electrochemical sulfur oxidation system 3 is provided with a water inlet 14 and a water outlet 15; the anode cover plate 10 and the anode electrode 11 are sealed and connected through a silica gel gasket, and the cathode cover plate 13 and the cathode electrode 12 are sealed and connected through a silica gel gasket. The anode electrode 11 and the cathode electrode 12 are connected to titanium wires 21 and 22 respectively, and are sealed and connected through silica gel gaskets. The titanium wires 21 and 22 are connected to the battery booster module system 2 through external wires 18 .
本实施方式为克服含硫有机废水处理中存在的能源消耗、运行成本高及单质硫回收率低的技术难点，以降低系统的能源消耗、运行成本、提高单质硫的回收率为目的，构建了微生物燃料电池电能原位利用的含硫废水处理系统。该系统可以在室温下运行，硫酸盐去除率可达89%，单质硫回收率可达46%。通过该系统中的升压模块系统，可以在无外加能量输入的情况下，驱动电化学硫氧化系统实现硫化物向单质硫的转化，从而实现了电能的原位利用。该系统解决了含硫废水处理过程中的高能耗、低单质硫回收率问题，实现了含硫废水的资源化及能源化利用。本实施方式可利用系统中自身产生的能量来驱动电化学系统，因此，本系统是一个能量零消耗的处理系统，可适用于实际含硫废水的处理。In order to overcome the technical difficulties of energy consumption, high operation cost and low recovery rate of elemental sulfur in the treatment of sulfur-containing organic wastewater, this implementation mode aims to reduce energy consumption and operation cost of the system and improve the recovery rate of elemental sulfur. Sulfur-containing wastewater treatment system utilizing microbial fuel cell electricity in situ. The system can operate at room temperature, the sulfate removal rate can reach 89%, and the elemental sulfur recovery rate can reach 46%. Through the step-up module system in the system, the electrochemical sulfur oxidation system can be driven to realize the conversion of sulfide to elemental sulfur without external energy input, thereby realizing the in-situ utilization of electric energy. The system solves the problems of high energy consumption and low recovery rate of elemental sulfur in the treatment process of sulfur-containing wastewater, and realizes the resource utilization and energy utilization of sulfur-containing wastewater. In this embodiment, the energy generated by the system itself can be used to drive the electrochemical system. Therefore, this system is a treatment system with zero energy consumption, which is applicable to the treatment of actual sulfur-containing wastewater.
本实施方式的微生物燃料电池电能原位利用的含硫废水处理系统的运行方式如下：该系统由3部分组成，其3组分的运行模式分别为：The operation mode of the sulfur-containing wastewater treatment system utilizing microbial fuel cell electric energy in situ in this embodiment is as follows: the system is composed of 3 parts, and the operation modes of the 3 components are respectively:
硫酸盐还原系统：以稳定运行的微生物燃料电池反应器的出水作为菌源，启动硫酸盐还原微生物燃料电池，阴阳极间以设定的外电阻启动（100-1000Ω），监测系统的电压输出情况，当输出电压稳定运行后（输出电压的在2-3个周期内达到稳定），向系统中添加市售的硫酸盐还原细菌作为硫酸盐还原系统的菌源，利用市售的硫酸盐还原细菌还原系统中的硫酸盐，利用产电细菌，在微生物燃料电池系统中获得电能。产生的电能输入到电池升压模块系统中进行贮存和累积。Sulfate reduction system: use the effluent of the microbial fuel cell reactor in stable operation as the bacterial source, start the sulfate reduction microbial fuel cell, start with the set external resistance (100-1000Ω) between the cathode and anode, and monitor the voltage output of the system , when the output voltage runs stably (the output voltage reaches stability within 2-3 cycles), add commercially available sulfate-reducing bacteria to the system as the bacterial source of the sulfate-reducing system, and use commercially available sulfate-reducing bacteria Reduction of sulfate in the system and use of electrogenic bacteria to obtain electrical energy in microbial fuel cell systems. The generated electrical energy is input into the battery booster module system for storage and accumulation.
电池升压模块系统：由计时继电器、电容等组成。通过计时继电器来控制电容器的充、放电的时间。利用不同容量的电容器以及不同数量的电容器，对硫酸盐还原微生物燃料电池系统产生的能量进行累加，以达到电化学硫氧化系统所需要的能量需求。Battery boost module system: composed of timing relays, capacitors, etc. The charging and discharging time of the capacitor is controlled by a timing relay. Capacitors with different capacities and different numbers of capacitors are used to accumulate the energy generated by the sulfate reduction microbial fuel cell system to meet the energy demand required by the electrochemical sulfur oxidation system.
电化学硫氧化系统：该系统为电化学反应系统，该系统由阳极、阴极和电解液组成。电解液为硫酸盐还原系统的出水。通过电池升压模块系统对硫酸盐还原系统收集的电能进行贮存和转化后，将升压模块作为外部电源供给到电化学硫氧化系统中，利用阳极发生的反应将电化学硫氧化系统中的S2-转化为单质硫。单质硫富集在阳极极板上，以便于快速收集产生的单质硫。Electrochemical sulfur oxidation system: This system is an electrochemical reaction system, which is composed of anode, cathode and electrolyte. The electrolyte is the effluent of the sulfate reduction system. After storing and converting the electric energy collected by the sulfate reduction system through the battery booster module system, the booster module is used as an external power supply to the electrochemical sulfur oxidation system. 2- Conversion to elemental sulfur. Elemental sulfur is enriched on the anode plate, so that the generated elemental sulfur can be collected quickly.
具体实施方式二：本实施方式与具体实施方式一不同的是：所述的阳极电极5和阳极电极11的材质为碳材料或金属材料。其它与具体实施方式一相同。Embodiment 2: This embodiment differs from Embodiment 1 in that: the material of the anode electrode 5 and the anode electrode 11 is carbon material or metal material. Others are the same as in the first embodiment.
具体实施方式三：本实施方式与具体实施方式一或二不同的是：所述的碳材料为碳纸、碳布、碳纤维刷、碳毡、玻璃碳、碳纳米管、石墨或石墨烯；所述的金属材料为不锈钢网、不锈钢板、钛板或钛网。其它与具体实施方式一或二相同。Specific embodiment three: the difference between this embodiment and specific embodiment one or two is that: the carbon material is carbon paper, carbon cloth, carbon fiber brush, carbon felt, glassy carbon, carbon nanotubes, graphite or graphene; The metal material mentioned is stainless steel mesh, stainless steel plate, titanium plate or titanium mesh. Others are the same as in the first or second embodiment.
具体实施方式四：本实施方式与具体实施方式一至三之一不同的是：所述的阴极电极6和阴极电极12材质为碳纸、碳布、碳纤维刷、碳毡、玻璃碳、碳纳米管、石墨、石墨烯、不锈钢网、不锈钢板、钛板或钛网。其它与具体实施方式一至三之一相同。Specific embodiment four: this embodiment is different from one of specific embodiments one to three in that: the cathode electrode 6 and the cathode electrode 12 are made of carbon paper, carbon cloth, carbon fiber brush, carbon felt, glassy carbon, carbon nanotubes , graphite, graphene, stainless steel mesh, stainless steel plate, titanium plate or titanium mesh. Others are the same as those in the first to third specific embodiments.
具体实施方式五：本实施方式与具体实施方式一至四之一不同的是：所述的硫酸盐还原微生物燃料电池系统1由若干个串联或并联一起，然后通过外部导线18与电池升压模块系统2连接。其它与具体实施方式一至四之一相同。Embodiment 5: This embodiment differs from Embodiment 1 to Embodiment 4 in that: the sulfate reducing microbial fuel cell system 1 is connected in series or in parallel, and then connected to the battery booster module system through an external wire 18 2 connections. Others are the same as one of the specific embodiments 1 to 4.
具体实施方式六：本实施方式与具体实施方式一至五之一不同的是：所述的硫酸盐还原微生物燃料电池系统1通过外部导线18与电池升压模块系统2连接，然后将电池升压模块系统2进行串联或并联。其它与具体实施方式一至五之一相同。Embodiment 6: The difference between this embodiment and one of Embodiments 1 to 5 is that the sulfate-reducing microbial fuel cell system 1 is connected to the battery boost module system 2 through an external wire 18, and then the battery boost module System 2 is connected in series or in parallel. Others are the same as one of the specific embodiments 1 to 5.
具体实施方式七：本实施方式与具体实施方式一至六之一不同的是：所述的电化学硫氧化系统3与电池升压模块系统2连接方式为一对多或多对一的连接方式。其它与具体实施方式一至六之一相同。Embodiment 7: This embodiment differs from Embodiments 1 to 6 in that the electrochemical sulfur oxidation system 3 is connected to the battery booster module system 2 in a one-to-many or many-to-one connection. Others are the same as one of the specific embodiments 1 to 6.
具体实施方式八：本实施方式的一种微生物燃料电池电能原位利用的硫酸盐处理系统的方法，其处理方法操作如下：将含硫废水通过进水口8注入到硫酸盐还原微生物燃料电池系统1中，在设定的固定外阻下，启动硫酸盐还原微生物燃料电池，利用该系统中的硫酸盐还原菌代谢硫酸盐，将硫酸盐转化成硫化物，产生的电能通过电池升压模块系统2进行能量的收集和捕获，存储和利用，将硫酸盐还原微生物燃料电池系统1中处理的出水通过出水口9注入到电化学硫氧化系统3中，利用来自升压模块系统2储存的电能，驱动电化学硫氧化系统3发生反应，从而实现硫化物向单质硫的转化。Embodiment 8: A method for a sulfate treatment system for in-situ utilization of microbial fuel cell electric energy in this embodiment, the treatment method is as follows: inject sulfur-containing wastewater into the sulfate reduction microbial fuel cell system 1 through the water inlet 8 , under the set fixed external resistance, start the sulfate-reducing microbial fuel cell, use the sulfate-reducing bacteria in the system to metabolize sulfate, convert sulfate into sulfide, and generate electricity through the battery booster module system 2 Collect and capture, store and utilize energy, inject the effluent treated in the sulfate reduction microbial fuel cell system 1 into the electrochemical sulfur oxidation system 3 through the water outlet 9, and use the electric energy stored in the booster module system 2 to drive The electrochemical sulfur oxidation system 3 reacts to realize the conversion of sulfide to elemental sulfur.
具体实施方式九：本实施方式与具体实施方式八不同的是：所述的硫酸盐还原微生物燃料电池系统1和电化学硫氧化系统3的进水方式为续批式的进水方式或连续流进水方式。其它与具体实施方式八相同。Embodiment 9: The difference between this embodiment and Embodiment 8 is that the water inlet mode of the sulfate reducing microbial fuel cell system 1 and the electrochemical sulfur oxidation system 3 is a continuous batch type water inlet mode or a continuous flow Water intake method. Others are the same as the eighth embodiment.
具体实施方式十：本实施方式与具体实施方式九或八不同的是：所述的固定外阻的阻值为100-1000Ω。其它与具体实施方式九或八相同。Embodiment 10: This embodiment is different from Embodiment 9 or Embodiment 8 in that: the resistance value of the fixed external resistance is 100-1000Ω. Others are the same as Embodiment 9 or Embodiment 8.
通过以下试实施例证本发明的有益效果：The beneficial effects of the present invention are illustrated by the following test examples:
实施例一Embodiment one
本实施例的一种微生物燃料电池电能原位利用的硫酸盐处理系统，由硫酸盐还原微生物燃料电池系统1、电池升压模块系统2和电化学硫氧化系统3构成，硫酸盐还原微生物燃料电池系统1与电化学硫氧化系统3分别通过外部导线18与电池升压模块系统2连接；A sulfate treatment system for in-situ utilization of microbial fuel cell electric energy in this embodiment is composed of a sulfate reducing microbial fuel cell system 1, a battery boost module system 2 and an electrochemical sulfur oxidation system 3. The sulfate reducing microbial fuel cell System 1 and electrochemical sulfur oxidation system 3 are respectively connected to battery booster module system 2 through external wires 18;
所述的硫酸盐还原微生物燃料电池系统1由阳极盖板4、阳极电极5、阴极电极6、阴极盖板7、进水口8和出水口9构成，其中，阳极盖板4与阳极电极5固定连接，阴极盖板7与阴极电极6固定连接，阴极电极6、阳极电极5分别通过外部导线18与电池升压模块系统2连接；The sulfate reducing microbial fuel cell system 1 is composed of an anode cover plate 4, an anode electrode 5, a cathode electrode 6, a cathode cover plate 7, a water inlet 8 and a water outlet 9, wherein the anode cover plate 4 is fixed to the anode electrode 5 connection, the cathode cover plate 7 is fixedly connected to the cathode electrode 6, and the cathode electrode 6 and the anode electrode 5 are respectively connected to the battery booster module system 2 through external wires 18;
所述的电化学硫氧化系统3由阳极盖板10、阳极电极11、阴极电极12、阴极盖板13、进水口14和出水口15构成，其中，阳极盖板10与阳极电极11固定连接，阴极盖板13与阴极电极12固定连接，阳极电极11与阴极电极12分别通过外部导线18与电池升压模块系统2连接。The electrochemical sulfur oxidation system 3 is composed of an anode cover plate 10, an anode electrode 11, a cathode electrode 12, a cathode cover plate 13, a water inlet 14 and a water outlet 15, wherein the anode cover plate 10 is fixedly connected to the anode electrode 11, The cathode cover plate 13 is fixedly connected to the cathode electrode 12 , and the anode electrode 11 and the cathode electrode 12 are respectively connected to the battery booster module system 2 through external wires 18 .
本实施例一种微生物燃料电池电能原位利用的硫酸盐处理系统的操作方法如下：将含硫废水16通过进水口8注入到硫酸盐还原微生物燃料电池系统1中，启动硫酸盐还原微生物燃料电池，在设定的固定外阻下（100-1000Ω），监测系统的电压输出情况，当输出电压稳定运行后（输出电压的在2-3个周期内达到稳定），加入的硫酸盐还原菌代谢硫酸盐，将硫酸盐转化成硫化物，产生的电能通过电池升压模块系统2进行能量的收集和捕获，存储和利用，将硫酸盐还原微生物燃料电池系统1中处理的出水通过出水口9注入到电化学硫氧化系统3中，利用来自升压模块系统2储存的电能，驱动电化学硫氧化系统3发生反应，将电化学硫氧化系统3处理的水17排出，从而实现硫化物向单质硫的转化。The operating method of a sulfate treatment system for in-situ utilization of microbial fuel cell electric energy in this embodiment is as follows: inject sulfur-containing wastewater 16 into the sulfate-reducing microbial fuel cell system 1 through the water inlet 8, and start the sulfate-reducing microbial fuel cell , under the set fixed external resistance (100-1000Ω), monitor the voltage output of the system, when the output voltage is stable (the output voltage is stable within 2-3 cycles), the added sulfate-reducing bacteria metabolize Sulfate, converting sulfate into sulfide, the generated electric energy is collected, captured, stored and utilized through the battery booster module system 2, and the effluent treated in the sulfate reduction microbial fuel cell system 1 is injected through the water outlet 9 In the electrochemical sulfur oxidation system 3, use the electric energy stored in the booster module system 2 to drive the electrochemical sulfur oxidation system 3 to react, and discharge the water 17 treated by the electrochemical sulfur oxidation system 3, so as to realize the conversion of sulfide to elemental sulfur transformation.
实施例二废水处理过程中COD的去除效果The removal effect of COD in the waste water treatment process of embodiment two
化学需氧量（COD）作为水体受污染程度的综合性指标之一，是废水处理过程需要重点监测的指标。启动微生物燃料电池电能原位利用的含硫废水处理系统，在室温下运行实施例一的系统并考察系统的运行情况。该系统的COD的降解情况，见图2。由图2可知，在不同的反应批次内，该系统均能实现82%的COD去除率，在反应的3个批次内，COD去除率稳定，表明系统运行状况良好，具有很好的平行性。以上结果表明，该系统在废水处理过程中，具有良好的处理性能。Chemical oxygen demand (COD), as one of the comprehensive indicators of the degree of water pollution, is an indicator that needs to be monitored in the process of wastewater treatment. Start the sulfur-containing wastewater treatment system for in-situ utilization of microbial fuel cell electric energy, run the system of Example 1 at room temperature and investigate the operation of the system. The COD degradation of the system is shown in Figure 2. It can be seen from Figure 2 that in different reaction batches, the system can achieve a COD removal rate of 82%. In the three reaction batches, the COD removal rate is stable, indicating that the system is in good condition and has good parallelism. sex. The above results show that the system has good treatment performance in the process of wastewater treatment.
实施例三废水处理过程中硫酸盐的去除效果The removal effect of sulfate in the waste water treatment process of embodiment three
对于含硫废水处理系统而言，首先需要考察的是含硫废水中的硫酸盐的去除效果。本实施例分别考察采用实施例一的方法，不同的反应批次内的硫酸盐的去除率，见图3。由图3可知，在3个连续的反应批次内，该系统可以实现89%的硫酸盐去除率，高的硫酸盐去除率表明，该系统可以有效的处理含硫废水，并且处理性能稳定。For the sulfur-containing wastewater treatment system, the first thing to examine is the removal effect of sulfate in the sulfur-containing wastewater. This embodiment examines respectively adopting the method of embodiment one, the removal rate of the sulfate in different reaction batches, see Fig. 3. It can be seen from Figure 3 that the system can achieve a sulfate removal rate of 89% in three consecutive reaction batches. The high sulfate removal rate indicates that the system can effectively treat sulfur-containing wastewater and has stable treatment performance.
实施例四含硫废水处理系统中电能的原位利用Example 4 In-situ Utilization of Electric Energy in Sulfur-Containing Wastewater Treatment System
利用电池升压模块系统，将微生物燃料电池硫酸盐还原系统中捕获的电能进行贮存和升压，然后应用在电化学硫氧化系统中，图4监测了实施例一中的电化学升压模块系统中贮存的电能应用在电化学硫氧化系统中的放电情况。通过采用不同的电容器个数，进行充、放电，在电池升压模块系统中获得了较高的电能贮存。在电化学硫氧化放电系统中，通过升压模块的放电，可以获得不同的氧化电流，可以为后续的电化学硫氧化系统的运行提供足够的电能。Using the battery boost module system, the electrical energy captured in the microbial fuel cell sulfate reduction system is stored and boosted, and then applied to the electrochemical sulfur oxidation system. Figure 4 monitors the electrochemical boost module system in Example 1 The electrical energy stored in the battery is applied to the discharge of the electrochemical sulfur oxidation system. By adopting different numbers of capacitors for charging and discharging, higher electric energy storage is obtained in the battery booster module system. In the electrochemical sulfur oxidation discharge system, different oxidation currents can be obtained through the discharge of the booster module, which can provide sufficient electric energy for the subsequent operation of the electrochemical sulfur oxidation system.
实施例五含硫废水处理系统中单质硫的回收率The recovery rate of elemental sulfur in the sulfur-containing wastewater treatment system of embodiment five
实施例一中利用电化学升压模块提供的电能，电化学硫氧化系统可以在无需外部能量输入的条件下发生反应。本实施例考察实施例一中反应运行的不同批次内的单质硫的回收情况，见图5。由图5可知，不同批次的试验结果表明，该系统可实现46%的单质硫回收率。该系统可方便快捷的将沉积在阳极上的单质硫进行有效的回收利用，从而实现了含硫废水中硫酸盐资源的资源化利用。在该系统的运行过程中，无外加的能量输入，因此，该系统是一个能量自供给的处理系统，具有可实现废水资源化、能源化利用的技术优势，因此，该系统可广泛的应用于含硫废水的处理过程中。In Embodiment 1, by using the electric energy provided by the electrochemical booster module, the electrochemical sulfur oxidation system can react without external energy input. This embodiment investigates the recovery of elemental sulfur in different batches of the reaction operation in the first embodiment, as shown in FIG. 5 . It can be seen from Figure 5 that the test results of different batches show that the system can achieve a recovery rate of elemental sulfur of 46%. The system can conveniently and quickly recycle the elemental sulfur deposited on the anode effectively, thereby realizing the resource utilization of sulfate resources in sulfur-containing wastewater. During the operation of the system, there is no external energy input. Therefore, the system is a self-supplied energy treatment system, which has the technical advantages of realizing waste water recycling and energy utilization. Therefore, the system can be widely used in During the treatment of sulfur-containing wastewater.
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